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We consider electronic excitation induced with a continuous wave laser to an excited bound state which can predissociate due to a radiationless transition to a dissociative state. The conditions for a separation of the process into the preparation of a vibrational eigenstate which subsequently dissociates due to a radiationless transition are established. We point out that the probability of the radiationless transition can be calculated from a time‐dependent nuclear autocorrelation function, an expression which nicely reflects the pictorial aspect of the Franck–Condon principle.

Dynamic aspects of electronic predissociation